A Thiourea Competitive Crystallization Strategy for FA‐Based Perovskite Solar Cells

Abstract The solution process of perovskite solar cells may lead to widespread defects in the device, causing severe nonradiative recombination and the loss of conversion efficiency. Herein, a strategy of embedding thiourea into perovskite to manipulate the crystallization process and passivate the defects simultaneously is demonstrated. A competitive crystallization mechanism by embedding thiourea into perovskite has been proposed for the improvement of morphology and crystallinity. The defects in the device have been dramatically decreased by the strong coordination of CS bond in thiourea with the undercoordinated Pb 2+ . Moreover, the bilateral affinity of thiourea to the SnO 2 and perovskite can enhance the interface contact by the bridging bonding, which will release the residual stress of perovskite films. As a result, the thiourea‐embedding device achieves a power conversion efficiency over 24% and shows excellent storage and illumination stabilities. Even undergoing 3768 h storage, the maximum efficiency value of unencapsulated device keeps over 94%. Furthermore, the efficiency of the optimized device maintains over 80% after 120 h continuous illumination at 60 °C.